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The effects of a low-temperature ZnTe buffer layer on the crystallinity and surface roughness of ZnTe epilayers grown on (100) GaAs substrates by metalorganic vapor phase epitaxy are investigated. X-ray rocking curves, Raman spectra, and atomic force microscopy analysis results prove that both the crystallinity and surface roughness of ZnTe epilayers can be markedly improved by introducing a lowtemperature ZnTe buffer layer, and that the thickness of the low-temperature ZnTe buffer layer is critical for obtaining a high-crystallinity ZnTe epilayer with a smooth surface.